Host model uncertainties in aerosol radiative forcing estimates: results from the AeroCom Prescribed intercomparison study

Simulated multi-model “diversity” in aerosol direct radiative forcing estimates is often perceived as a measure of aerosol uncertainty. However, current models used for aerosol radiative forcing calculations vary considerably in model components relevant for forcing calculations and the associated “host-model uncertainties” are generally convoluted with the actual aerosol uncertainty. In this AeroCom Prescribed intercomparison study we systematically isolate and quantify host model uncertainties on aerosol forcing experiments through prescription of identical aerosol radiative properties in twelve participating models. Even with prescribed aerosol radiative properties, simulated clear-sky and all-sky aerosol radiative forcings show significant diversity. For a purely scattering case with globally constant optical depth of 0.2, the global-mean all-sky top-of-atmosphere radiative forcing is −4.47Wm−2 and the inter-model standard deviation is 0.55Wm−2, corresponding to a relative standard deviation of 12 %. For a case with partially absorbing aerosol with an aerosol optical depth of 0.2 and single scattering albedo of 0.8, the forcing changes to 1.04Wm−2, and the standard deviation increases to 1.01W−2, corresponding to a significant relative standard deviation of 97 %. However, the top-of-atmosphere forcing variability owing to absorption (subtracting the scattering case from the case with scattering and absorption) is low, with absolute (relative) standard deviations of 0.45Wm−2 (8 %) clear-sky and 0.62Wm−2 (11 %) all-sky. Scaling the forcing standard deviation for a purely scattering case to match the sulfate radiative forcing in the Aero- Com Direct Effect experiment demonstrates that host model uncertainties could explain about 36% of the overall sulfate forcing diversity of 0.11Wm−2 in the AeroCom Direct Radiative Effect experiment.

A multimodel assessment of the influence of regional anthropogenic emission reductions on aerosol direct radiative forcing and the role of intercontinental transport

In this study, we assess changes of aerosol optical depth (AOD) and direct radiative forcing (DRF) in response to the reduction of anthropogenic emissions in four major pollution regions in the Northern Hemisphere by using results from nine global models in the framework of the Hemispheric Transport of Air Pollution (HTAP). DRF at top of atmosphere (TOA) and surface is estimated based on AOD results from the HTAP models and AOD-normalized DRF (NDRF) from a chemical transport model. The multimodel results show that, on average, a 20% reduction of anthropogenic emissions in North America, Europe, East Asia, and South Asia lowers the global mean AOD (all-sky TOA DRF) by 9.2% (9.0%), 3.5% (3.0%), and 9.4% (10.0%) for sulfate, particulate organic matter (POM), and black carbon (BC), respectively. Global annual average TOA all-sky forcing efficiency relative to particle or gaseous precursor emissions from the four regions (expressed as multimodel mean ± one standard deviation) is  ±3.5 ±0.8,  ±4.0 ±1.7, and 29.5 ±18.1mWm ±2 per Tg for sulfate (relative to SO2), POM, and BC, respectively. The impacts of the regional emission reductions on AOD and DRF extend well beyond the source regions because of intercontinental transport (ICT). On an annual basis, ICT accounts for 11 ±5% to 31 ±9% of AOD and DRF in a receptor region at continental or subcontinental scale, with domestic emissions accounting for the remainder, depending on regions and species. For sulfate AOD, the largest ICT contribution of 31 ±9% occurs in South Asia, which is dominated by the emissions from Europe. For BC AOD, the largest ICT contribution of 28 ±18% occurs in North America, which is dominated by the emissions from East Asia. The large spreads among models highlight the need to improve aerosol processes in models, and evaluate and constrain models with observations.

Radiative forcing of climate by hydrochlorofluorocarbons and hydrofluorocarbons

We measure infrared absorption spectra of 18 hydrochlorofluorocarbons and hydrofluorocarbons, seven of which do not yet appear in the literature. The spectra are used in a narrowband model of the terrestrial infrared radiation to calculate radiative forcing and global warming potentials. We investigate the sensitivity of the radiative forcing to the absorption spectrum temperature dependence, halocarbon vertical profile, stratospheric adjustment, cloudiness, spectral overlap, and latitude, and we make some recommendations for the reporting of radiative forcings that would help to resolve discrepancies between assessments. We investigate simple methods of estimating instantaneous radiative forcing directly from a molecule's absorption spectrum and we present a new method that agrees to within 0.3% with our narrowband model results.

Radiative forcing and global warming potentials of 11 halogenated compounds

Radiative forcing values have been calculated for 11 halogenated compounds which are in current use or which have been suggested as possible replacements for the chlorofluorocarbons. Absorption cross-sections measured over a range of atmospheric temperature and pressure conditions as part of a multi-laboratory programme have been used together with a narrow band radiative transfer model. We provide a “best estimate” radiative forcing taking into account the likely vertical profile of the gas in each case. The Global Warming Potential over a variety of time horizons has also been calculated where the lifetime is available. We present the first such information for 1,2-dichloroethane. For chloroform our radiative forcing is 5 times higher than the value used in previous assessments, possibly because these ignored the effect of absorption outside the 800–1200 cm−1 “window”. For several of the other compounds considered here, our forcing is between 10 and 30% lower than previous assessments. The perfluorocarbons have been found to have large global warming potentials, many times that of CFC-11, due to both strong absorption and long lifetimes. The importance of absorption features at wavenumbers below 800 cm−1 and the effect of temperature variations in absorption cross-section on the radiative forcing are also investigated.

Updated radiative forcing estimates of 65 halocarbons and nonmethane hydrocarbons

The direct radiative forcing of 65 chlorofluorocarbons, hydrochlorofluorocarbons, hydrofluorocarbons, hydrofluoroethers, halons, iodoalkanes, chloroalkanes, bromoalkanes, perfluorocarbons and nonmethane hydrocarbons has been evaluated using a consistent set of infrared absorption cross sections. For the radiative transfer models, both line-by-line and random band model approaches were employed for each gas. The line-by-line model was first validated against measurements taken by the Airborne Research Interferometer Evaluation System (ARIES) of the U.K. Meteorological Office; the computed spectrally integrated radiance of agreed to within 2% with experimental measurements. Three model atmospheres, derived from a three-dimensional climatology, were used in the radiative forcing calculations to more accurately represent hemispheric differences in water vapor, ozone concentrations, and cloud cover. Instantaneous, clear-sky radiative forcing values calculated by the line-by-line and band models were in close agreement. The band model values were subsequently modified to ensure exact agreement with the line-by-line model values. Calibrated band model radiative forcing values, for atmospheric profiles with clouds and using stratospheric adjustment, are reported and compared with previous literature values. Fourteen of the 65 molecules have forcings that differ by more than 15% from those in the World Meteorological Organization [1999] compilation. Eleven of the molecules have not been reported previously. The 65-molecule data set reported here is the most comprehensive and consistent database yet available to evaluate the relative impact of halocarbons and hydrocarbons on climate change.

Sensitivity of direct radiative forcing by mineral dust to particle characteristics

Airborne dust affects the Earth's energy balance — an impact that is measured in terms of the implied change in net radiation (or radiative forcing, in W m-2) at the top of the atmosphere. There remains considerable uncertainty in the magnitude and sign of direct forcing by airborne dust under current climate. Much of this uncertainty stems from simplified assumptions about mineral dust-particle size, composition and shape, which are applied in remote sensing retrievals of dust characteristics and dust-cycle models. Improved estimates of direct radiative forcing by dust will require improved characterization of the spatial variability in particle characteristics to provide reliable information dust optical properties. This includes constraints on: (1) particle-size distribution, including discrimination of particle subpopulations and quantification of the amount of dust in the sub-10 µm to <0.1 µm mass fraction; (2) particle composition, specifically the abundance of iron oxides, and whether particles consist of single or multi-mineral grains; (3) particle shape, including degree of sphericity and surface roughness, as a function of size and mineralogy; and (4) the degree to which dust particles are aggregated together. The use of techniques that measure the size, composition and shape of individual particles will provide a better basis for optical modelling.

Radiative forcing effect of ice-age dust

During glacial periods, dust deposition rates and inferred atmospheric concentrations were globally much higher than present. According to recent model results, the large enhancement of atmospheric dust content at the last glacial maximum (LGM) can be explained only if increases in the potential dust source areas are taken into account. Such increases are to be expected, due to effects of low precipitation and low atmospheric (CO2) on plant growth. Here the modelled three-dimensional dust fields from Mahowald et al. and modelled seasonally varying surface-albedo fields derived in a parallel manner, are used to quantify the mean radiative forcing due to modern (non-anthropogenic) and LGM dust. The effect of mineralogical provenance on the radiative properties of the dust is taken into account, as is the range of optical properties associated with uncertainties about the mixing state of the dust particles. The high-latitude (poleward of 45°) mean change in forcing (LGM minus modern) is estimated to be small (–0.9 to +0.2 W m–2), especially when compared to nearly –20 W m–2 due to reflection from the extended ice sheets. Although the net effect of dust over ice sheets is a positive forcing (warming), much of the simulated high-latitude dust was not over the ice sheets, but over unglaciated regions close to the expanded dust source region in central Asia. In the tropics the change in forcing is estimated to be overall negative, and of similarly large magnitude (–2.2 to –3.2 W m–2) to the radiative cooling effect of low atmospheric (CO2). Thus, the largest long-term climatic effect of the LGM dust is likely to have been a cooling of the tropics. Low tropical sea-surface temperatures, low atmospheric (CO2) and high atmospheric dust loading may be mutually reinforcing due to multiple positive feedbacks, including the negative radiative forcing effect of dust.

The dependence of radiative forcing and feedback on evolving patterns of surface temperature change in climate models

Experiments with CO2 instantaneously quadrupled and then held constant are used to show that the relationship between the global-mean net heat input to the climate system and the global-mean surface-air-temperature change is nonlinear in Coupled Model Intercomparison Project phase 5 (CMIP5) Atmosphere-Ocean General Circulation Models (AOGCMs). The nonlinearity is shown to arise from a change in strength of climate feedbacks driven by an evolving pattern of surface warming. In 23 out of the 27 AOGCMs examined the climate feedback parameter becomes significantly (95% confidence) less negative – i.e. the effective climate sensitivity increases – as time passes. Cloud feedback parameters show the largest changes. In the AOGCM-mean approximately 60% of the change in feedback parameter comes from the topics (30N-30S). An important region involved is the tropical Pacific where the surface warming intensifies in the east after a few decades. The dependence of climate feedbacks on an evolving pattern of surface warming is confirmed using the HadGEM2 and HadCM3 atmosphere GCMs (AGCMs). With monthly evolving sea-surface-temperatures and sea-ice prescribed from its AOGCM counterpart each AGCM reproduces the time-varying feedbacks, but when a fixed pattern of warming is prescribed the radiative response is linear with global temperature change or nearly so. We also demonstrate that the regression and fixed-SST methods for evaluating effective radiative forcing are in principle different, because rapid SST adjustment when CO2 is changed can produce a pattern of surface temperature change with zero global mean but non-zero change in net radiation at the top of the atmosphere (~ -0.5 Wm-2 in HadCM3).

Global analysis of radiative forcing from fire-induced shortwave albedo change

Land surface albedo, a key parameter to derive Earth's surface energy balance, is used in the parameterization of numerical weather prediction, climate monitoring and climate change impact assessments. Changes in albedo due to fire have not been fully investigated on a continental and global scale. The main goal of this study, therefore, is to quantify the changes in instantaneous shortwave albedo produced by biomass burning activities and their associated radiative forcing. The study relies on the MODerate-resolution Imaging Spectroradiometer (MODIS) MCD64A1 burned-area product to create an annual composite of areas affected by fire and the MCD43C2 bidirectional reflectance distribution function (BRDF) albedo snow-free product to compute a bihemispherical reflectance time series. The approximate day of burning is used to calculate the instantaneous change in shortwave albedo. Using the corresponding National Centers for Environmental Prediction (NCEP) monthly mean downward solar radiation flux at the surface, the global radiative forcing associated with fire was computed. The analysis reveals a mean decrease in shortwave albedo of −0.014 (1σ = 0.017), causing a mean positive radiative forcing of 3.99 Wm−2 (1σ = 4.89) over the 2002–20012 time period in areas affected by fire. The greatest drop in mean shortwave albedo change occurs in 2002, which corresponds to the highest total area burned (378 Mha) observed in the same year and produces the highest mean radiative forcing (4.5 Wm−2). Africa is the main contributor in terms of burned area, but forests globally give the highest radiative forcing per unit area and thus give detectable changes in shortwave albedo. The global mean radiative forcing for the whole period studied (~0.0275 Wm−2) shows that the contribution of fires to the Earth system is not insignificant.

Radiative forcing and climate metrics for ozone precursor emissions: the impact of multi-model averaging

Multi-model ensembles are frequently used to assess understanding of the response of ozone and methane lifetime to changes in emissions of ozone precursors such as NOx, VOCs (volatile organic compounds) and CO. When these ozone changes are used to calculate radiative forcing (RF) (and climate metrics such as the global warming potential (GWP) and global temperature-change potential (GTP)) there is a methodological choice, determined partly by the available computing resources, as to whether the mean ozone (and methane) concentration changes are input to the radiation code, or whether each model's ozone and methane changes are used as input, with the average RF computed from the individual model RFs. We use data from the Task Force on Hemispheric Transport of Air Pollution source–receptor global chemical transport model ensemble to assess the impact of this choice for emission changes in four regions (East Asia, Europe, North America and South Asia). We conclude that using the multi-model mean ozone and methane responses is accurate for calculating the mean RF, with differences up to 0.6% for CO, 0.7% for VOCs and 2% for NOx. Differences of up to 60% for NOx 7% for VOCs and 3% for CO are introduced into the 20 year GWP. The differences for the 20 year GTP are smaller than for the GWP for NOx, and similar for the other species. However, estimates of the standard deviation calculated from the ensemble-mean input fields (where the standard deviation at each point on the model grid is added to or subtracted from the mean field) are almost always substantially larger in RF, GWP and GTP metrics than the true standard deviation, and can be larger than the model range for short-lived ozone RF, and for the 20 and 100 year GWP and 100 year GTP. The order of averaging has most impact on the metrics for NOx, as the net values for these quantities is the residual of the sum of terms of opposing signs. For example, the standard deviation for the 20 year GWP is 2–3 times larger using the ensemble-mean fields than using the individual models to calculate the RF. The source of this effect is largely due to the construction of the input ozone fields, which overestimate the true ensemble spread. Hence, while the average of multi-model fields are normally appropriate for calculating mean RF, GWP and GTP, they are not a reliable method for calculating the uncertainty in these fields, and in general overestimate the uncertainty.

Radiative forcing and climate change

Aviation causes climate change as a result of its emissions of CO2, oxides of nitrogen, aerosols, and water vapor. One simple method of quantifying the climate impact of past emissions is radiative forcing. The radiative forcing due to changes in CO2 is best characterized, but there are formidable difficulties in estimating the non-CO2 forcings – this is particularly the case for possible aviation-induced changes in cloudiness (AIC). The most recent comprehensive assessment gave a best estimate of the 2005 total radiative forcing due to aviation of about 55–78 mW m−2 depending on whether AIC was included or not, with an uncertainty of at least a factor of 2. The aviation CO2 radiative forcing represents about 1.6% of the total CO2 forcing from all human activities. It is estimated that, including the non-CO2 effects, aviation contributes between 1.3 and 14% of the total radiative forcing due to all human activities. Alternative methods for comparing the future impact of present-day aviation emissions are presented – the perception of the relative importance of the non-CO2 emissions, relative to CO2, depends considerably on the chosen method and the parameters chosen within those methods.

Small global-mean cooling due to volcanic radiative forcing

In both the observational record and atmosphere-ocean general circulation model (AOGCM) simulations of the last ∼∼ 150 years, short-lived negative radiative forcing due to volcanic aerosol, following explosive eruptions, causes sudden global-mean cooling of up to ∼∼ 0.3 K. This is about five times smaller than expected from the transient climate response parameter (TCRP, K of global-mean surface air temperature change per W m−2 of radiative forcing increase) evaluated under atmospheric CO2 concentration increasing at 1 % yr−1. Using the step model (Good et al. in Geophys Res Lett 38:L01703, 2011. doi:10.​1029/​2010GL045208), we confirm the previous finding (Held et al. in J Clim 23:2418–2427, 2010. doi:10.​1175/​2009JCLI3466.​1) that the main reason for the discrepancy is the damping of the response to short-lived forcing by the thermal inertia of the upper ocean. Although the step model includes this effect, it still overestimates the volcanic cooling simulated by AOGCMs by about 60 %. We show that this remaining discrepancy can be explained by the magnitude of the volcanic forcing, which may be smaller in AOGCMs (by 30 % for the HadCM3 AOGCM) than in off-line calculations that do not account for rapid cloud adjustment, and the climate sensitivity parameter, which may be smaller than for increasing CO2 (40 % smaller than for 4 × CO2 in HadCM3).

Airborne measurements of the spectral surface albedo over Morocco and its influence on the radiative forcing of Saharan dust

This PhD thesis is embedded into the DFG research project SAMUM, the Saharan Mineral Dust Experiment which was initiated with the goal to investigate the optical and microphysical properties of Saharan dust aerosol, its transport, and its radiative effect. This work described the deployment of the Spectral Modular Airborne Radiation Measurement SysTem (SMART-Albedometer) in SAMUM after it has been extended in its spectral range. The SAMUM field campaign was conducted in May and June 2006 in south-eastern Morocco. At two ground stations and aboard two aircraft various measurements in an almost pure plume of Saharan dust were conducted. Airborne measurements of the spectral upwelling and downwelling irradiance are used to derive the spectral surface albedo in its typical range in the experiment region. Typical spectral types are presented and compared to the surface albedo derived from MISR satellite data. Furthermore, the radiative forcing of the observed Saharan dust is estimated in dependence on the surface albedo and its regional variations. A strong dependence of the radiative forcing not only on the surface albedo, but also on the optical properties of the dust aerosol is observed. It is unique to SAMUM that all these influential parameters have been measured in near-source Saharan dust, which made the calculations shown in this work possible.

The impact of ice crystals on radiative forcing and remote sensing of arctic boundary-layer mixed-phase clouds

This PhD thesis is embedded into the Arctic Study of Tropospheric Aerosol, Clouds and Radiation (ASTAR) and investigates the radiative transfer through Arctic boundary-layer mixed-phase (ABM) clouds. For this purpose airborne spectral solar radiation measurements and simulations of the solar and thermal infrared radiative transfer have been performed. This work reports on measurements with the Spectral Modular Airborne Radiation measurement sysTem (SMART-Albedometer) conducted in the framework of ASTAR in April 2007 close to Svalbard. For ASTAR the SMART-Albedometer was extended to measure spectral radiance. The development and calibration of the radiance measurements are described in this work. In combination with in situ measurements of cloud particle properties provided by the Laboratoire de M¶et¶eorologie Physique (LaMP) and simultaneous airborne lidar measurements by the Alfred Wegener Institute for Polar and Marine Research (AWI) ABM clouds were sampled. The SMART-Albedometer measurements were used to retrieve the cloud thermodynamic phase by three different approaches. A comparison of these results with the in situ and lidar measurements is presented in two case studies. Beside the dominating mixed-phase clouds pure ice clouds were found in cloud gaps and at the edge of a large cloud field. Furthermore the vertical distribution of ice crystals within ABM clouds was investigated. It was found that ice crystals at cloud top are necessary to describe the observed SMART-Albedometer measurements. The impact of ice crystals on the radiative forcing of ABM clouds is in vestigated by extensive radiative transfer simulations. The solar and net radiative forcing was found to depend on the ice crystal size, shape and the mixing ratio of ice crystals and liquid water droplets.